The morphology of interface hydration products is crucial as it directly determines the interface mechanics. Inspired by the fishing nets, we employed photo-grafted active copolymer Poly(vinylpyrrolidone-co-acrylic acid) on the inert glass fibers. Providing a template for PVP-co-PAA maintains its regulatory capability in cement paste. For the first time, ordered nanomesh-like hydrated calcium silicate (CSH) with average pore diameter of 30 nm are developed in cement paste. The interface strength and energy absorption increased by 90 % and 253 %, respectively. XPS and SEM revealed that the multi-scale regulation mechanisms originated from the preferential adsorption and stable dispersion of Ca result from the strong electronegativity and steric hindrance of pyrrolidone rings. CSH nuclei (60 nm) dispersed well on fiber templates, stacked along fiber surfaces, without collapse or tilt, intertwined into nanomesh. Nanomesh-like CSH in cement paste holds significant potentials for the improvement of mechanical properties of fiber-cement interfaces, contributing to construction sustainability.